Silicon-containing aluminum nitride particles, sintered body, resin composition, and method for producing silicon-containing aluminum nitride particles

Abstract

Silicon-containing aluminum nitride particles contain a ratio of a total of a mass of aluminum and a mass of nitrogen of 90% by mass or more, and a ratio of a mass of silicon of 1.5% by mass or more and 10.0% by mass or less relative to a total of the mass of aluminum and the mass of silicon, as obtained by analyzing particles using an inductively coupled plasma-atomic emission spectroscope, and a mass of oxygen and the mass of nitrogen, as obtained by analyzing the particles using an oxygen/nitrogen analyzer, being 100% by mass, wherein a ratio (X/Y) is 0.40 or more and 0.85 or less, a ratio of the mass of oxygen is denoted as X % by mass, a specific surface area of the particles, as measured according to a BET method, is denoted as Y m 2 /g.

What is claimed is: 
     
         1 . Silicon-containing aluminum nitride particles comprising:
 a ratio of a total of a mass of aluminum and a mass of nitrogen of 90% by mass or more, and a ratio of a mass of silicon of 1.5% by mass or more and 10.0% by mass or less relative to a total of the mass of aluminum and the mass of silicon, as obtained by analyzing particles using an inductively coupled plasma-atomic emission spectroscope, and a mass of oxygen and the mass of nitrogen, as obtained by analyzing the particles using an oxygen/nitrogen analyzer, being 100% by mass,   wherein a ratio (X/Y) of a numerical value X of the X % by mass to a numerical value Y of the Y m 2 /g is 0.40 or more and 0.85 or less, a ratio of the mass of oxygen is denoted as X % by mass, a specific surface area of the particles, as measured according to a BET method, is denoted as Y m 2 /g.   
     
     
         2 . Silicon-containing aluminum nitride particles comprising:
 a ratio of a total of a mass of aluminum and a mass of nitrogen of 90% by mass or more, and a ratio of a mass of silicon of 1.5% by mass or more and 10.0% by mass or less relative to a total of the mass of aluminum and the mass of silicon, as obtained by analyzing particles using an inductively coupled plasma-atomic emission spectroscope, and a mass of oxygen and the mass of nitrogen, as obtained by analyzing the particles using an oxygen/nitrogen analyzer, being 100% by mass,   wherein a ratio O P /N P  of an oxygen atomic percentage O P  to a nitrogen atomic percentage N P , as obtained by analyzing the particles according to X-ray photoelectron spectroscopy, is more than 2.0.   
     
     
         3 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a ratio of the mass of oxygen is 0.9% by mass or more and 3.5% by mass or less relative to the total of the mass of aluminum, the mass of silicon, the mass of nitrogen, and the mass of oxygen being 100% by mass. 
     
     
         4 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a specific surface area of the particles, as measured according to a BET method, is 2.5 m 2 /g or more and 4.5 m 2 /g or less. 
     
     
         5 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a ratio of the mass of silicon is 1.5% by mass or more and 4.0% by mass or less relative to the total of the mass of aluminum, the mass of silicon, the mass of nitrogen, and the mass of oxygen being 100% by mass. 
     
     
         6 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein a ratio Al Ka /N Ka  of a peak intensity Al Ka  of aluminum Ka rays to a peak intensity N Ka  of nitrogen Ka rays, as obtained by analyzing the particles according to X-ray fluorescence spectrometry, is more than 740. 
     
     
         7 . The silicon-containing aluminum nitride particles according to  claim 1 , having a composition represented by Al 1-x Si x N and comprising oxygen, wherein x satisfies 0.02≤x≤0.2. 
     
     
         8 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein an average particle diameter, as measured according to a Fisher Sub-Sieve Sizer method, is 0.1 μm or more and 100 μm or less. 
     
     
         9 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein an average particle diameter, as measured according to a Fisher Sub-Sieve Sizer method, is 0.5 μm or more and 3.0 μm or less. 
     
     
         10 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein an average particle diameter, as measured according to a Fisher Sub-Sieve Sizer method, is more than 3.0 μm and 80 μm or less. 
     
     
         11 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein in a powder X-ray diffraction pattern measured using CuKa rays (1.5418 Å), a peak intensity at a diffraction angle 2θ of 43.3°±0.5° is 5% or less relative to a peak intensity at a diffraction angle 2θ of 33.2°±0.5° being 100%. 
     
     
         12 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a reflectance for light having a wavelength range of 380 nm or more and 730 nm or less is 50% or more. 
     
     
         13 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a reflectance for light having a wavelength range of 380 nm or more and 730 nm or less is 80% or more. 
     
     
         14 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein a reflectance for light having a wavelength of 250 nm is 40% or less. 
     
     
         15 . The silicon-containing aluminum nitride particles according to  claim 1 , wherein when 1.0 g of the silicon-containing aluminum nitride particles is brought into contact with 50 mL of a boiled 6 mol/L hydrochloric acid aqueous solution, an amount of ammonia generated in the hydrochloric acid aqueous solution is 120 ppm by mass or less. 
     
     
         16 . The silicon-containing aluminum nitride particles according to  claim 2 , having a composition represented by Al 1-x Si x N and comprising oxygen, wherein x satisfies 0.02≤x≤0.2. 
     
     
         17 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein an average particle diameter, as measured according to a Fisher Sub-Sieve Sizer method, is 0.1 μm or more and 100 μm or less. 
     
     
         18 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein in a powder X-ray diffraction pattern measured using CuKa rays (1.5418 Å), a peak intensity at a diffraction angle 2θ of 43.3°±0.5° is 5% or less relative to a peak intensity at a diffraction angle 2θ of 33.2°±0.5° being 100%. 
     
     
         19 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein a reflectance for light having a wavelength range of 380 nm or more and 730 nm or less is 50% or more. 
     
     
         20 . The silicon-containing aluminum nitride particles according to  claim 2 , wherein a reflectance for light having a wavelength of 250 nm is 40% or less. 
     
     
         21 . A sintered body comprising the silicon-containing aluminum nitride particles according to  claim 1 . 
     
     
         22 . A resin composition comprising the silicon-containing aluminum nitride particles according to  claim 1  and a resin. 
     
     
         23 . A sintered body comprising the silicon-containing aluminum nitride particles according to  claim 2 . 
     
     
         24 . A resin composition comprising the silicon-containing aluminum nitride particles according to  claim 2  and a resin. 
     
     
         25 . A method for producing silicon-containing aluminum nitride particles comprising:
 mixing aluminum nitride and silicon nitride to obtain a raw material mixture containing silicon nitride in an amount of 2% by mass or more and 15% by mass or less relative to a total of aluminum nitride and silicon nitride being 100% by mass;   subjecting the raw material mixture to a first heat treatment at a pressure of 0.101 MPa or more and a temperature of 1,600° C. or higher and 2,100° C. or lower to obtain a first heat-treated product; and   subjecting the obtained first heat-treated product to a second heat treatment at a temperature of 850° C. or higher and lower than 1,000° C. to obtain a second heat-treated product.   
     
     
         26 . The method for producing silicon-containing aluminum nitride particles according to  claim 25 , further comprising wet dispersing the first heat-treated product prior to the second heat treatment. 
     
     
         27 . The method for producing silicon-containing aluminum nitride particles according to  claim 25 , further comprising subjecting the first heat-treated product to the second heat treatment in an oxygen-containing atmosphere for 1 hour or more and 15 hours or less. 
     
     
         28 . The method for producing silicon-containing aluminum nitride particles according to  claim 26 , further comprising: subjecting the first heat-treated product to solid-liquid separation after the wet dispersion; and drying the product in a temperature range of 80° C. or higher and 120° C. or lower. 
     
     
         29 . The method for producing silicon-containing aluminum nitride particles according to  claim 26 , wherein a particle diameter ratio D/Dm of an average particle diameter D, as obtained by measuring the first heat-treated product after the wet dispersion according to a Fisher Sub-Sieve Sizer method, to a volume median diameter Dm, as obtained by measuring the first heat-treated product after the wet dispersion according to a laser diffraction particle size distribution measurement method, is 0.2 or more and 0.5 or less. 
     
     
         30 . The method for producing silicon-containing aluminum nitride particles according to  claim 26 , wherein a particle diameter ratio D/Dm of an average particle diameter D, as obtained by measuring the first heat-treated product after the wet dispersion according to a Fisher Sub-Sieve Sizer method, to a volume median diameter Dm, as obtained by measuring the first heat-treated product after the wet dispersion according to a laser diffraction particle size distribution measurement method, is 0.55 or more and 0.95 or less. 
     
     
         31 . The method for producing silicon-containing aluminum nitride particles according to  claim 25 , wherein the second heat-treated product comprises silicon-containing aluminum nitride particles having a ratio of a total of a mass of aluminum and a mass of nitrogen of 90% by mass or more, and a ratio of a mass of silicon of 1.5% by mass or more and 10.0% by mass or less relative to a total of the mass of aluminum and the mass of silicon, as obtained by analyzing the particles using an inductively coupled plasma-atomic emission spectroscope, and the mass of nitrogen and a mass of oxygen, as obtained by analyzing the particles using an oxygen/nitrogen analyzer, being 100% by mass,
 wherein a ratio (X/Y) of a numerical value X of the X % by mass to a numerical value Y of the Y m 2 /g is 0.40 or more and 0.85 or less, a ratio of the mass of oxygen is denoted as X % by mass, a specific surface area of the particles, as measured according to a BET method, is denoted as Y m 2 /g.   
     
     
         32 . The method for producing silicon-containing aluminum nitride particles according to  claim 25 , wherein the second heat-treated product comprises silicon-containing aluminum nitride particles having a ratio of a total of a mass of aluminum and a mass of nitrogen of 90% by mass or more, and a ratio of a mass of silicon of 1.5% by mass or more and 10.0% by mass or less relative to a total of the mass of aluminum and the mass of silicon, as obtained by analyzing the particles using an inductively coupled plasma-atomic emission spectroscope, and the mass of nitrogen and a mass of oxygen, as obtained by analyzing the particles using an oxygen/nitrogen analyzer, being 100% by mass,
 wherein a ratio O P /N P  of an oxygen atomic percentage O P  to a nitrogen atomic percentage N P , as obtained by analyzing the particles according to X-ray photoelectron spectroscopy, is more than 2.0.